Cited by 57CO2 Sequestration and Geologic InteractionsSubcritical and Supercritical Water ProcessesCarbon dioxide utilization in catalysis

Critical Water Coverage during Forsterite Carbonation in Thin Water Films: Activating Dissolution and Mass Transport

Open access
Placencia-Gómez, Edmundo, Kerisit, Sebastien N., Mehta, Hardeep S., Qafoku, Odeta, Thompson, Christopher J., Graham, Trent R., Ilton, Eugene S., Loring, John S.·2020·Environmental Science & Technology

Abstract

In geologic carbon sequestration, CO 2 is injected into geologic reservoirs as a supercritical fluid (scCO 2 ). The carbonation of divalent silicates exposed to humidified scCO 2 occurs in angstroms to nanometers thick adsorbed H 2 O films. A threshold H 2 O film thickness is required for carbonate precipitation, but a mechanistic understanding is lacking. In this study, we investigated carbonation of forsterite (Mg 2 SiO 4 ) in humidified scCO 2 (50 °C and 90 bar), which serves as a model system for understanding subsurface divalent silicate carbonation reactivity. Attenuated total reflection infrared spectroscopy pinpointed that magnesium carbonate precipitation begins at 1.5 monolayers of adsorbed H 2 O. At about this same H 2 O coverage, transmission infrared spectroscopy showed that forsterite dissolution begins and electrical impedance spectroscopy demonstrated that diffusive transport accelerates. Molecular dynamics simulations indicated that the onset of diffusion is due to an abrupt decrease in the free-energy barriers for lateral mobility of outer-spherically adsorbed Mg 2+ . The dissolution and mass transport controls on divalent silicate reactivity in wet scCO 2 could be advantageous for maximizing permeability near the wellbore and minimize leakage through the caprock.

Integrity signals

Registry

Crossref · 10.1021/acs.est.0c00897

Cites

93 of 93 references verified0 citation errors · 0 not checkable

Statistics

Recomputing p-values needs the paper’s full text.

Claims the paper makes

The text we found for this paper looks like another document, so its claims and self-check weren’t run. The registry and citation checks still apply.

Self-check

Percentages, sums and reported differences re-computed from the paper’s own numbers.

The text we found for this paper looks like another document, so the self-check wasn’t run.

Cites

Flagged first, then by citations

Research works printed but not linked: 8

  1. [4]4. Boulet-Audet, M.; Buffeteau, T.; Boudreault, S.; Daugey, N.; Pézolet, M. Quantitative determination of band distortions in diamond attenuated total reflectance infrared spectra, J. Phys. Chem. B 2010, 114, 8255-8261.
  2. [5]5. Harrick, N. J. Internal Reflection Spectroscopy; John Wiley & Sons: New York, 1967.
  3. [6]6. Bertie, J. E.; Eysel, H. H. Infrared intensities of liquids I: Determination of infrared optical and dielectric constants by FT-IR using the CIRCLE ATR cell, Appl. Spectrosc. 1985, 39, 392-401.
  4. [7]7. Bertie, J. E.; Zhang, S. L.; Manji, R. Infrared intensities of liquids X: Accuracy of current methods of obtaining optical constants from multiple attenuated total reflection measurements using the CIRCLE cell, Appl. Spectrosc. 1992, 46, 1660-1665.
  5. [8]8. Ohta, K.; Ishida, H. Matrix formalism for calculation of electric field intensity of light in stratified multilayered films, Appl. Opt. 1990, 29, 1952-1959.
  6. [9]9. Loring, J. S.; Land, D. P. Theoretical determination of parameters for optimum surface specificity in overlayer attenuated-total-reflection infrared spectroscopy, Appl. Opt. 1998, 37, 3515- 3526.
  7. [11]11. de Juan, A.; Tauler, R. Multivariate curve resolution (MCR) from 2000: Progress in concepts and applications, Crit. Rev. Anal. Chem. 2006, 36, 163-176.
  8. [12]12. Yeşilbaş, M.; Boily, J.-F. Thin ice films at mineral surfaces, J. Phys. Chem. Lett. 2016, 7, 2849-2855.

Cited by

Sorted by citations

Authors
Placencia-Gómez, E., Kerisit, S. N., Mehta, H. S., Qafoku, O., Thompson, C. J., Graham, T. R., Ilton, E. S., & Loring, J. S.
Affiliations
  • University of Liège (BE)
  • Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  • Pacific Northwest National Laboratory (US)
Corresponding author
Loring, John S.
Venue
Environmental Science & Technology
Published
2020-05-08
Volume
54
Issue
11
Pages
6888-6899
ISSN
  • 0013-936X (ISSN-L)
  • 1520-5851
OpenAlex
W3022034930
Cited by
57
References
93
Citations by year
2026: 9 · 2025: 15 · 2024: 15 · 2023: 5 · 2022: 7 · 2021: 5 · 2020: 1
FWCI
1.62
Type
journal article
Language
en
Open access
Locations
  • Environmental Science & Technology (publishedVersion)
  • PubMed (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders
Basic Energy Sciences
Topics
  • Physical Sciences › Environmental Science › Environmental Engineering › CO2 Sequestration and Geologic Interactions
  • Physical Sciences › Engineering › Biomedical Engineering › Subcritical and Supercritical Water Processes
  • Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
Keywords
supercritical carbon dioxide, adsorbed water films, magnesium carbonate precipitation, mass transfer, activation barrier, geologic carbon sequestration, carbonate precipitation
MeSH terms
Carbon Dioxide, Carbonates, Solubility, Water, Silicon Compounds

About these checks

Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.

Statistics and arithmetic are recomputed, not judged.

Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.

What counts as a claim ›How we measure confidence ›How we check this ›

Are you an author, or do you see a problem with this page? Request a review